From quantum to classical dipole plasmon resonances in highly-doped nano-crystals

TL;DR

This paper investigates the transition from quantum to classical dipole plasmon resonances in highly-doped ZnO nano-crystals, demonstrating how size influences resonance behavior and validating a quantum model with RPA calculations.

Contribution

It introduces a quantum model validated by RPA calculations to explain the size-dependent transition of plasmon resonances in doped nano-crystals.

Findings

Smooth transition from quantum to classical resonance with increasing size

Quantum model accurately predicts experimental trends

Resonance tunable from visible to infra-red

Abstract

Dipole plasmon resonances are ubiquitous in nano-particles with delocalized charge carriers. Doped semi-conductor colloidal nano-crystals constitute a novel paradigm for plasmon excitations in a finite electron system and offer the possibility to tune the carrier density and thus the dipole resonance from visible to infra-red, which cannot be achieved with metallic clusters. Restricting ourselves to highly n-doped ZnO nano-crystals, we explain the observed smooth transition from small sizes dominated by quantum effects to large sizes where the resonance reaches its classical value. A schematic two interacting highly degenerate level quantum model, validated by a full Random Phase Approximation calculation, yields nicely the experimentally observed trends.